Raman spectra of solid CH4 under high pressure. III. New high pressure phases in solid CH4 and CD4

Abstract
We have observed the Raman spectra of the intramolecular vibrations in solid CH4 and CD4 at T=4.2 K under high pressure. For solid CH4, the spectra changed markedly at P≂9 kbar, indicative of a new phase VI above this pressure. For solid CD4, an analogous change was observed at P≂5.4 kbar, indicating a phase transition from phase III to a new phase IV. The spectra of these new phases, CH4 VI and CD4 IV, are very similar so that it is concluded that the crystal structures of the phases are isomorphous. The observed spectra seem to indicate that the molecular orientations of methane molecules in the new high pressure phases are fully ordered.

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